期刊
ACS APPLIED NANO MATERIALS
卷 5, 期 3, 页码 3521-3530出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsanm.1c04151
关键词
molybdenum disulfide; sulfur vacancy; selenium doping; hydrogen evolution reaction; density functional theory
资金
- National Natural Science Foundation of China [21872048]
This article introduces a defect-predesigned strategy to produce MoS2 with single-atomic S vacancies by preparing Se-doped MoS2 and subsequent removing the Se. The results show that MoS2 with an optimal concentration of S vacancies exhibits outstanding HER performance.
The consensus has been built on the fact that the hydrogen evolution reaction (HER) activity of MoS2 basal planes can be activated by S vacancies. Currently, the popular strategy for fabricating S vacancies is to remove part of S atoms of MoS2. Owing to the same identity of S atoms, the removal process is usually random and does not have selectivity. Herein, we develop a defect-predesigned strategy to produce MoS2 with single-atomic S vacancies (SV-MoS2) simply by preparing Se-doped MoS2 (Se-MoS2) and subsequent removing the Se of Se-MoS2. S vacancies originates from the vaporization of the doped Se atoms, making the formation of S vacancies have a high selectivity and raising a good possibility for precisely modulating the concentration of S vacancies. The results show that the concentration of S vacancies can be controlled over the range from similar to 7.46% to 13.54%. MoS1.76 with similar to 12.10% of S vacancies exhibits outstanding HER performance: an overpotential of 100 mV at 10 mA cm(-2) and a Tafel slope of 49 mV dec(-1), corroborating the theoretical prediction about the optimum concentration of S vacancies. Density functional theory calculation further reveals that the activation of MoS2 basal planes may intrinsically originate from the modification of S vacancies to band structure and density of state of MoS2, optimizing the hydrogen adsorption energy. This defect-predesigned strategy reduces the probability of forming the aggregates of S vacancies and will be more helpful for understanding how S vacancies affect the properties of MoS2.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据